Positive Feedback‐Driven NiRu Frustrated Lewis Pairs Catalyst Enables a Self‐Reinforcing Catalytic Cycle for Cascade‐Coupled Hydrogen Production

Abstract The alkaline hydrogen evolution reaction (HER) associated with anion exchange membrane water electrolyzers (AEMWEs) is kinetically hindered by sluggish water dissociation and complex intermediate adsorption, which previous reports have inadequately addressed through isolated optimization, neglecting the intrinsic coupling between HER elementary steps. Herein, we report a frustrated Lewis pairs (FLPs) catalyst comprising NiRu dual single‐atoms and adjacent NiRu nanoclusters anchored on nitrogen‐doped carbon (Ni 1 Ru 1 ‐NiRu@NC), mimicking the enzymatic positive feedback mechanism that drives a self‐reinforcing catalytic cycle and accelerates the coupled elementary steps in a cascade manner. The catalyst featuring spatially proximate Lewis acid and base sites enable sequential reaction steps, where water dissociation occurs at acid sites and hydrogen adsorption proceed at base sites. The two steps are bridged through rapid hydrogen spillover channel, constructing a closed catalytic circuit in which hydrogen consumption at base sites promotes continuous water dissociation at acid sites. Benefiting from this positive feedback loop, Ni 1 Ru 1 ‐NiRu@NC achieves a remarkable HER performance and exhibits exceptional long‐term durability (>1000 h at 1.0 A cm − 2 ) in AEMWEs. Our findings demonstrate a new strategy to integrate positive feedback‐driven, cascade‐coupled catalysis in FLPs systems, offering a promising pathway toward high‐performance alkaline HER catalysts for industrial application.